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A series of mononuclear Ru(II) complexes of the type [Ru(S)2(K)]2+, where S = 1,10-phenanthroline/2,2′-bipyridine and K = 4-OH-btsz, 4-CH3-btsz, 3,4-di-OCH3-btsz, 4-OH-binh, 4-CH3-binh, 3,4-di-OCH3-binh, were prepared and characterized by elemental analysis, FTIR, 1H-NMR, and mass spectroscopy. The complexes displayed metal–ligand charge transfer (MLCT) transitions in the visible region. These ligands formed bidentate octahedral ruthenium complexes. The title complexes were evaluated for their in vivo anticancer activity against a transplantable murine tumor cell line, Ehrlisch’s ascites carcinoma (EAC), and in vitro cytotoxic activity against human cancer cell lines Molt 4/C8 and CEM and murine tumor cell line L1210. The ruthenium complexes showed promising biological activity especially in decreasing tumor volume and viable ascites cell counts. Treatment with these complexes prolonged the life span of mice bearing EAC tumors by 10–52%. In vitro evaluation of these ruthenium complexes revealed cytotoxic activity from 0.21 to 24 μM against Molt 4/C8, 0.16 to 19 μM aginst CEM, and 0.75 to 32 μM against L1210. [ABSTRACT FROM AUTHOR]